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Discusses the vibrational predissociation of the ammonia monomer ND [sub 3]-Ar through excitation of the 'umbrella' mode of ND [sub 3]. Effect of a simultaneous excitation of one of the Van der Waals modes on the lifetime of the complex and on the product state distribution; Final state distributions.

The time-dependent wave packet technique is applied to the Golden Rule treatment of vibrational predissociation. The wave packet at time zero is taken as the product of the quasibound wave function and the coupling inducing predissociation. The rate for vibrational predissociation can then be obtained by Fourier transform into the energy domain of the time-dependent wave packet autocorrelation function. The method has been applied to a model triatomic van der Waals molecule. It is shown that when the bound-state components of the wave packet are projected out, the time-dependent version of the Golden Rule approximation provides an alternative efficient technique to treat intramolecular decay. [ABSTRACT FROM AUTHOR]

A programming error, which affects many of the numbers, tables, and figures of the dissociation part of this paper, is corrected. It does not affect the results concerning the quasibound states. The main conclusions are unchanged, except that the correlation between final rotational distributions originating from the two components of the same tunneling doublet has become rather high. © 2001 American Institute of Physics. [ABSTRACT FROM AUTHOR]